Zant because his battle is just epic, having to use your gale boomerang, iron boots, double clawshots, ball and chain, finally ending down with a sword brawl. I was impressed to see the hurricane spin being used by zant, but I just countered it with the great spin
I would have to go with Vaati (Reborn form--tall Sorceror Form), Ganondorf (not his beast form--Ganon) from Twilight Princess, and Majora's Wrath. In my opinion, these are the coolest looking Main Zelda Villains, and they could kick almost anyones' butt. If for some reason one of those didn't count though, my fourth choice would be Shadow Link.
Vaati, Ganondorf and Majora. Vaati because he's so cool, and Ganondorf is super intense and epic. Majora is my favourite just because of how much mystery there is surrounding it and how powerful it is.